Developing an eco-friendly and effective approach for preparing N, S co-doped hierarchical porous carbons (NSHPC) for capacitive deionization (CDI) is a huge task for desalination. Herein, NSHPCSKK with interconnected hierarchical pore structures, manufactured via self-activation/co-activation of sodium lignosulfonate (SLS) encapsulation using KNO3-KHCO3 activators, inducing N, S co-doping. Different from NSHPCS and NSHPCSK, NSHPCSKK exhibits the highest specific surface area (SBET, 2264.67 m2/g) and a unique hierarchical pore structure (mesoporous volume/pore volume (Vmeso/ Vpore), 0.65). Small-angle X-ray scattering (SAXS) and scanning electron microscopy (SEM) both reveal the complex interconnected pore structure of NSHPCSKK. Regional Raman imaging conjugated with XPS reveals the presence of extensively distributed N, S co-doped defect structures, providing NSHPCSKK with excellent wettability and electrochemical performance. DFT calculations indicate that the N, S co-doping at the defect sites depicts excellent adsorption capability. Eventually, NSHPCSKK acquired an impressive salt adsorption capacity (SAC) of 20.5 mg/g and the highest average salt adsorption rate (ASAR) of 12.1 mg/g/min, indicating its superior desalting performance. In-situ Raman spectroscopy confirms NSHPCSKK’s rapid ion regeneration mechanism. The research introduces a span-new NSHPC synthesis strategy for fabricating advanced NSHPC with rapid desalination response for upgrading CDI desalination.
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